Vet. Med. Czech, 47, 2002 (6):

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1 Vet. Med. Czech, 47, 2002 (6): Original Paper Variations in environmental contamination by polychlorinated biphenyls (PCB) and chlorinated pesticides (Lindane, DDT) on pig farms in district in 1994 to 1999 R. ULRICH, J. RASZYK Veterinary Research Institute, Brno, ABSTRACT: Environmental samples (n = 216) were collected at regular intervals from 1994 to 1999 on three pig farms (D., M., T.) in the area of the district town of,. e samples of feed mixtures (n = 85), drinking water (n = 44), barn dust sediments (n = 45), and muscular tissue of feeder pigs (n = 42) were analysed for the concentrations of PCB (sum of 7 indicator congeners), DDT (sum of 6 isomers), and lindane (γ-hexachlorocyclohexane). e concentrations of lindane showed increasing tendencies in feed mixtures ( ), drinking water ( ), barn dust sediments ( ), and pork ( ). e limit of permissible concentrations (hereinafter limit) was exceeded in two samples of feed mixtures collected in e limit for DDT was exceeded in two samples of feed mixtures collected in Generally, the concentrations showed a decreasing tendency in feed mixtures and barn dust sediments ( ) and regular fluctuations in pork. e limit for PCB was exceeded in two samples of feed mixtures collected in 1994 and in one sample of drinking water collected in e concentrations showed increasing tendencies in feed mixtures ( ) and pork ( ). Decreasing tendencies were observed in drinking water ( ) and barn dust sediments ( ). Compared with mean values for the, the concentrations of lindane were higher in feed samples collected in 1994, 1997, and 1998, in drinking water samples collected in 1994 and 1995, and in pork samples collected in , the concentrations of DDT were higher in feed samples collected in 1994, 1997, and 1998, drinking water samples collected in 1995, and pork samples collected in 1994 and , and the concentrations of PCB were higher in feed samples collected in 1997 and 1998, in drinking water samples collected in 1994 and 1995, and in pork samples collected in e health risk of DDT, lindane, and PCB has been assessed as moderate, medium, and moderately increased, respectively. Keywords: pig farms; polychlorinated biphenyls; lindane; DDT; feed mixtures; drinking water; dust sediments; pork; sources; health risk e major pollution sources in the area under study, district,, are lignite mines, oil and natural gas sources, a large power plant, and intensive road traffic. e agriculture in this area is characterised by intensive animal (pig) and plant production including viticulture and fruit production. Records provided by the District Veterinary Administration at indicate that the power plant, combusting brown coal and lignite, was the most significant pollution source in the period of our monitoring. erefore, impacts of this environmental burden on pigs, as reflected in the contamination by highly dangerous organic pollutants (polychlorinated bi- Supported by the Ministry of Agriculture of the (Project MZe-M ), Ministry of the Environment of the (Project GA/1650/93) and Grant Agency of the (Grant No. 525/96/0924). 159

2 Original Paper Vet. Med. Czech, 47, 2002 (6): phenyls, chlorinated pesticides), were investigated on three farms located at distances of 6 km (farm D.), 10 km (farm M.), and 16 km (farm T.) from the district town. Partial results of continuing investigations done on the three farms and focussed on environmental mutagenic factors (Raszyk et al., 1995), occurrence of chlorinated pesticides and PCB in the farm environment (Raszyk et al., 1996a) and porcine tissues (Raszyk et al., 1996b), effects of the pollutants on the immune system (Raszyk et al., 1997), and differences between cattle and pig farms (Raszyk et al., 1998) were published previously. Results of quantitative studies of the transfer of PCBs from feed into tissues of fattened pigs were published by Vemmer et al. (1989, 1991). e contents of chlorinated pesticides and PCB in feeds for pigs in the period were monitored by Lovell et al. (1996). Glynn et al. (2000) studied possible regional differences in concentrations of PCBs and chlorinated pesticides in adipose tissues from pigs in the same period. is paper shows trends of concentrations of chlorinated pesticides and polychlorinated biphenyls in feed mixtures, drinking water, barn dust sediments, and muscular tissue of pigs and presents a comparison of the data obtained in the area of with available data from the remaining 80 districts of the. MATERIAL AND METHODS e analysed materials included samples of feed mixtures (n = 85), drinking water (n = 44), barn dust sediments (n = 45), and tissues of feeder pigs (n = 42) collected on three farms (D., M., T.) in district in 1994 to Farm characteristics Farm D. housed feeder pigs fed dry diets except for 2 barns where the liquid feeding system Funcki (Herning, Denmark) was installed. e pigs had unlimited access to drinkers supplied from a public water source. e materials collected on the farm consisted of 35 feed samples, 14 drinking water samples, 14 samples of barn dust sediments, and 14 samples of pork (77 samples in total). Farm M. housed feeder pigs fed liquid diets (system Schauer, Prambachkürchen, Austria). Water used for diet processing came from a private well. e premises were heated with natural gas. e materials collected on the farm included 25 feed samples, 18 samples of drinking water, 18 samples of barn dust, and 16 samples of pork (total 77 samples). Farm T. housed feeder pigs fed liquid diets (system Schauer, Prambachkürchen, Austria) and drinkers were at disposal. Water used for diet processing came from a public source. e materials collected on the farm included 25 feed samples, 12 water samples, 13 samples of barn dust sediments, and 12 samples of pork (total 62 samples). Sampling Dry feed samples (n = 85) were collected from feeding troughs (farm D.) or in the feed processing room (farms M. and T.). e minimum sample size was g. Drinking water samples (n = 44) were collected from drinkers or in the feed processing room (farm M.). e minimum sample volume was ml. Barn dust samples (n = 45) were collected from several sites in each barn using a vacuum cleaner. e mean sample weight was g. e retained dust was sieved through a 0.7 mm mesh and only particles passing through it (approx. 85% of the total amount) were analysed. Pork samples (n = 42) were collected from plantar muscles of the right thigh of slaughtered pigs (age 240 to 250 days, live weight 110 to 120 kg). e minimum sample size was g. Analytical methods Chlorinated pesticides and PCB were determined, after extraction with organic solvents and removal of co-extracts by absorption chromatography in activated Florisil columns, by HRGC using the gas chromatograph Varian Star 3600 CX (Varian, USA) and the 63 Ni electron capture detector (Gajdůšková and Ulrich, 1992). e final results were derived from standard calibration curves using the software Star Chromatography Workstation Version 5.0. e results were expressed as the sum of seven indicator PCB congeners (IUPAC Nos. 28, 52, 101, 118, 138, 153, 180) and the sum of six DDT isomers (o,p -DDE, p,p -DDE, o,p-ddd, p,p - DDD, o,p -DDT, p,p -DDT). Detection limit for 160

3 Vet. Med. Czech, 47, 2002 (6): Original Paper PCB was 50.0 ng/g and for lindane and DDT 10.0 ng/g; reproducibility for PCB, lindane and DDT was lower than 10.0%. e contamination of the feed mixtures, drinking water and pork was assessed according to the current Czech Regulations. No limits have been laid down for the content of pesticides and PCB in barn dust sediments so far. erefore we used our own internal limits that were 0.10 mg/kg for lindane and sum of DDT, and 0.20 mg/kg for PCB. Statistical data e results were processed using the software Stat Plus, Version 1.01 (Matoušková et al., 1992). To improve the meaningfulness, the data are presented in a) figures showing mean values only and allowing the assessment of trends and comparisons with mean values for the (when available), and b) tables showing the number of tested samples, arithmetic mean, ± S.D., and range (min. max.). In accordance with the binding methodology approved for the project GA/1650/93 by the Ministry of the Environment of the, the highest and the lowest numbers of samples were tested in 1994 and 1995, respectively. Mean concentrations of the pollutants in feed mixtures, drinking water, and pork were borrowed from the annual reports on contamination of food chains by xenobiotics in the (Valcl, 2000). Monitoring of chlorinated pesticides and PCB in drinking water by the State Veterinary Administration was discontinued in RESULTS e concentrations of lindane, DDT, and PCB in feed mixtures, drinking water, barn dust sediments, and pork are shown in Figures 1 through 12 and Tables 1 through 3. Lindane (Figures 1 4, Table 1) e statutory limit for lindane was exceeded in two samples of feed mixtures (0.177 and mg/kg) collected in An increase in lindane concentrations was observed in feed mixtures ( ), drinking water ( ), barn dust sediments ( ), and pork ( ). Compared with the mean values for the (Figures 1 4), the concentrations of lindane were higher in feed mixtures (1994, 1997 to 1999), drinking water (1994, 1995), and muscular tissue. Mean annual lindane concentrations ranged in feed samples from 1 54%, in drinking water samples from %, and in pork samples from 0.7 3% of the respective statutory limits (0.100 mg/kg, ng/l and 2.0 mg/kg fat, respectively) Figure 1. Lindane concentrations in commercial feeds for pigs (mg/kg) in district (n = 85) and a comparison with mean values for the Figure 2. Lindane concentrations in drinking water for pigs (ng/l) in district in (n = 44) and a comparison with mean values for drinking water for farm animals in the in

4 Original Paper Vet. Med. Czech, 47, 2002 (6): Table 1. Lindane concentrations in commercial feeds, drinking water, barn dust sediments, and pork of pigs fattened in district in n Mean SD Min. Max. Commercial feeds lindane (mg/kg) Drinking water lindane (ng/l) Barn dust sediments lindane (mg/kg) Pork lindane (mg/kg of fat) Figure 3. Lindane concentrations in barn dust sediments (mg/kg) collected on pig farms in district in (n = 45) Figure 4. Lindane concentrations in pork of pigs (mg/kg of fat) fattened in district (n = 42) and a comparison with mean values for the

5 Vet. Med. Czech, 47, 2002 (6): Original Paper DDT (Figures 5 8, Table 2) e limit for DDT was exceeded in three samples of feed mixtures collected in 1994 (0.054 and mg/kg) and in 1997 (0.064 mg/kg). Decreases in DDT concentrations were observed in feed mixtures and barn dust sediments (1997 to 1999). e concentration of DDT in muscular tissue fluctuated regularly. Compared with the mean for the (Figures 5 8), the concentrations of DDT were higher in feed mixtures (1994, 1997, 1998), drinking water (1995), and muscular tissue (1994, ). Mean annual DDT concentrations ranged in feed samples from 2 38%, in drinking water samples from % and in pork samples from 1.6 to 8.3% of the respective statutory limits (0.050 mg/ kg, ng/l and 1.0 mg/kg fat, respectively). PCB (Figures 9 12, Table 3) e limit for PCB was exceeded in two samples of feed mixtures (0.067 and mg/kg) in 1994 and in one sample of drinking water (63.3 ng/l) in Increases in PCB concentrations were observed in feed mixtures ( ), barn dust sediments ( ), and pork ( ). Decreasing tendencies of PCB concentrations were observed in drinking water ( ) and barn dust sediments ( ). Compared with the mean values for the (Figures 9 12), the concentrations of PCB were higher in feed mixtures (1997, 1998), drinking water (1994, 1995), and pork ( ). Mean annual PCB concentrations in feed samples ranged from 4 222%, in drinking water samples from 5 24%, and in pork samples from % Figure 5. DDT concentrations in commercial feeds for pigs (mg/kg) in district (n = 85) and a comparison with mean values for the Figure 6. DDT concentrations in drinking water for pigs (ng/l) in district in (n = 44) and a comparison with mean values for drinking water for farm animals in the in Figure 7. Concentrations of DDT in barn dust sediments (mg/kg) collected on swine farms in district in (n = 45) Figure 8. DDT concentrations in pork of pigs (mg/kg of fat) fattened in district (n = 42) and a comparison with mean values for the 163

6 Original Paper Vet. Med. Czech, 47, 2002 (6): Table 2. Sum of DDT concentrations in commercial feeds, drinking water, barn dust sediments, and pork of pigs fattened in district in n Mean SD Min. Max. Commercial feeds sum of DDT (mg/kg) Drinking water sum of DDT (ng/l) Barn dust sediments sum of DDT (mg/kg) Pork sum of DDT (mg/kg of fat) Figure 9. PCB concentrations in commercial feeds for pigs (mg/kg) in district (n = 85) and a comparison with mean values for the Figure 10. PCB concentrations in drinking water for pigs (ng/l) in district in (n = 44) and a comparison with mean values for drinking water for farm animals in the in

7 Vet. Med. Czech, 47, 2002 (6): Original Paper Table 3. Sum of PCB concentrations in commercial feeds, drinking water, barn dust sediments, and pork of pigs fattened in district in n Mean SD Min. Max. Commercial feeds sum of PCB (mg/kg) Drinking water sum of PCB (ng/l) Barn dust sediments sum of PCB (mg/kg) Pork sum of PCB (mg/kg of fat) Fig. 11. PCB concentrations in barn dust sediments (mg/kg) collected on pig farms in district in (n = 45) Figure 12. PCB concentrations in pork of pigs (mg/kg of fat) fattened in district (n = 42) and a comparison with mean values for the 165

8 Original Paper Vet. Med. Czech, 47, 2002 (6): of the respective statutory limits (0.050 mg/kg, 50 ng/l and 0.2 mg/kg fat, respectively). DISCUSSION Limits of permissible concentrations can be established in respect of 1) pollutant types; 2) sample types; 3) locations of farms. Analyses of 171 samples of feed mixtures, drinking water, and pork showed that the limits for PCB, DDT and lindane were exceeded in 3 (1.75%), 3 (1.75%) and 2 (1.17%) samples, respectively. In terms of sample types, the limits were exceeded in feed mixtures (7 of 85 samples; 8.2%) and in drinking water (1 of 44 samples; 2.3%). No exceeding was found in pork samples (n = 42). In terms of farms, the limits were exceeded on farm M. in 4 of the 59 tested samples (6.8%; 1 water and 3 feed samples), on farm D. in 3 of the 63 tested samples (4.8%; 3 feed samples) and on farm T. in 1 of the 49 tested samples (2.0%; 1 feed sample) Most of the excessive values were found in 1994 (n = 6) followed by 1995 and 1997 (n = 1). All samples collected in 1996 through 1999 were free of excessive concentrations of lindane and PCB. e lowest values relative to the limits were found for lindane and DDT in drinking water. e highest values relative to the limits were found for lindane, DDT, and PCB in feed samples. e lowest and the highest values relative to the limits for pork were found for lindane and PCB, respectively. e mean PCB concentration in pork (0.031 mg/kg) for 1999 is comparable with the mean (0.035 mg/kg) found within a monitoring in Belgium (Esposito et al., 2001). Data on the contamination of pork provide information on health risks associated with the consumption of this meat kind. Monitoring of organic pollutant concentrations in barn dust sediments provides the basic information for the assessment of indoor contamination rate in animal houses. Considering our internal limits for PCB (0.200 mg/kg), DDT (0.100 mg/ kg), and lindane (0.100 mg/kg) in barn dust sediments, excessive concentrations were found in 11 (24.4%), 7 (15.5%), and 2 (4.4%) of the 45 tested samples, respectively. All the 20 samples showing excessive concentrations were collected on farm M. Nevertheless, the limits for none of the three pollutants were exceeded in any pork sample collected from pigs fattened on this farm. Analyses of barn dust sediments proved to be a useful tool for the identification of pollution sources in our previous studies (Raszyk et al., 1998). us we were able to identify paint coats and capacitors as sources of PCB, imported fish meal and soy as sources of DDT, and the drug Fenoform forte used in the treatment of ectoparasitic infections as a source of lindane. It must be pointed out, however, that increased concentrations of pollutants in dust sediments need not be necessarily associated with increased concentrations in airborne particles (aerosol). e concentration of DDT in barn dust sediments paralleled its concentration in feed mixtures. erefore we can assume that the major source of DDT found in dust sediments was feed mixtures. No similar relation was found for lindane and PCB and these pollutants probably came from other major sources. DDT was used in the since 1945, and its use as an agricultural insecticide has been prohibited since DDT is still used in some African, Asian, and South American countries within the control of some insect-transmitted diseases (malaria, sleeping sickness) (Anonymous, 1995). Some feed components imported from such countries can be contaminated by DDT. Another source of DDT can be the contaminated soil around pig farms. DDT is known to persist in soil for more than 30 years (Aislabie et al., 1997). A part of it is degraded by biological processes and another part volatilises (Hawthorne et al., 1996). Fenoform forte (an antiectoparasitic drug containing 10% of lindane) at 1.5% concentration was used in district for the treatment of mange in pigs until Lindane-containing plant protection products (Lindan WP 80, Lindram 50/35) were used in district for the treatment of rape against Ceutorhynchids until Like DDT, contaminated feed can become a source of lindane for pigs. PCB produced by Chemko (Strážske, Slovakia) were used in the in the past. e manufacture was discontinued in 1984 and the use of PCB-containing paints was banned in the Czech Republic in e major sources of PCB identified on the pig farms included: 1. Old PCB-containing paint coats; if the paints contain more than 10 g of PCBs per 1 kg and animals have access to the painted construction parts, the concentration of PCB can exceed 10 mg/kg of fat. 166

9 Vet. Med. Czech, 47, 2002 (6): Original Paper 2. Old capacitors (as components of ventilators and fluorescent lamps) and transformer fillings; most of them have already been removed from the pig farms. 3. Occasional contamination of feed mixtures; the highest mean concentration of PCB in feed mixtures was found in the in 1994 (Delor 106, mg/kg). Hazardous components of feed mixtures include rendered fats and fish and meat-and-bone meals. Other possible sources of PCB include grit-coating plants, dumps of discarded capacitors and transformers, and PCB-contaminated mineral insulation oils. CONCLUSIONS e statutory limits of PCB, lindane and DDT were sporadically exceeded in feed samples collected in Moderately increasing tendencies were observed for lindane and PCB in feeds ( ), barn dust sediments ( ), and pork (lindane ; PCB ). Compared with mean values for the Czech Republic, pork produced in district contained more lindane, DDT (1994, ), and PCB ( ). Probable major sources of PCB, lindane and DDT on pig farms in district were identified. DDT insecticides, PCB-containing paints, and lindane as a plant protection product are no more used in district since 1974, 1986, and 1994, respectively. e results of the study are relevant to human preventive and occupational medicine. Acknowledgement e authors wish to thank to Dr. J. Salava and Dr. J. Palác (District Veterinary Administration,, ) for their helpful co-operation. Effective assistance of the State Veterinary Administration of the (supervisor Dr. J. Drápal) is appreciated. REFERENCES Aislabie J.M., Richards N.K., Boul H.L. (1997): Microbial degradation of DDT and its residues A review. N. Z. J. Agric. Res., 40, Anonymous (1995): Use of DDT in vector control. Bull. WHO, 73, Esposito M., Imparato E., Castellano V., Serpe L. (2001): Distribution of polychlorinated biphenyls in contaminated swine tissue. Vet. Hum. Toxicol., 43, Gajdůšková V., Ulrich R. (1992): Analysis of specific polychlorinated biphenyl congeners for the examination of raw materials and foodstuffs of animal origin (in Czech).Vet. Med. Czech, 37, Glynn A.W., Wernroth L., Atuma S., Linder C.E., Aune M., Nilsson I., Darnerud P.O. (2000): PCB and chlorinated pesticide concentrations in swine and bovine adipose tissue in Sweden : spatial and temporal trends. Sci. Total Environ., 246, Hawthorne S.B., Miller D.J., Louie P.K.K.. Butler R.D., Mayer G.G. (1996): Vapour-phase and particulate-associated pesticides and PCB concentrations in eastern North Dakota air samples. J. Environ. Quality, 25, Lovell R.A, Mc Chesney D.G., Price W.D. (1996): Organohalogen and organophosphorus pesticides in mixed feed rations: findings from FDA s domestic surveillance during fiscal years J. AOAC Int., 78, Matoušková O., Chalupa J., Cigler M., Hruška K. (1992): Stat plus Manual (in Czech). Brno, Veterinary Research Institute. 168 pp. Raszyk J., Pokorná Z., Strnadová Z., Gajdůšková V., Ulrich R., Jarošová A., Salava J., Palác J. (1995): Mutagenicity of stable dust and drinking water on swine and cattle farms. Vet. Med. Czech, 40, Raszyk J., Gajdůšková V., Ulrich R., Jarošová A., Šabatová V., Salava J., Palác J. (1996a): Occurrence of chlorinated pesticides and polychlorinated biphenyls in the stable and outside stable environment of farms for fattening (in Czech). Vet. Med. Czech, 41, Raszyk J., Gajdůšková V., Ulrich R., Nezveda K., Jarošová A., Šabatová V., Dočekalová H., Salava J., Palác J. (1996b): Evaluation of the presence of harmful pollutants in fattened pigs (in Czech). Vet. Med. Czech, 41, Raszyk J., Toman M., Gajdůšková V., Nezveda K., Ulrich R., Jarošová A., Dočekalová H., Salava J., Palác J. (1997): Effects of environmental pollutants on the porcine and bovine immune systems. Vet. Med. Czech, 42, Raszyk J., Ulrich R., Nápravník A., Salava J., Palác J. (1998): Differences in burden of pig and cattle farms by hazardous pollutants (Abstract).Vet. Med. Czech, 43,

10 Original Paper Vet. Med. Czech, 47, 2002 (6): Valcl O. (ed.) (2000): Contamination of Food Chains by Xenobiotics in the. State in 1999 (in Czech). Inf. Bull. SVS ČR, 1/99. Vemmer H., Heeschen W., Bluthgen A. (1989): Transfer of polychlorinated-biphenyls (PCB) from feed into tissues of fattening pigs. 1. e content of PCB in tissues of fattening pigs as related to the concentration of PCB in feed. Landbauforsch. Volk., 39, Vemmer H., Heeschen W., Bluthgen A. (1991): Transfer of polychlorinated-biphenyls (PCB) from feed into tissues of growing fattening pigs. 2. e quantitative transfer of PCB from feed to growing fattening pigs. Landbauforsch. Volk., 41, Received: Accepted after corrections: Corresponding Author Ing. Robert Ulrich, Veterinary Research Institute, Hudcova 70, Brno, Tel , fax , ulrich@vri.cz 168